CN105119019B - A kind of electrolyte and the lithium ion battery using the electrolyte - Google Patents
A kind of electrolyte and the lithium ion battery using the electrolyte Download PDFInfo
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- CN105119019B CN105119019B CN201510582081.5A CN201510582081A CN105119019B CN 105119019 B CN105119019 B CN 105119019B CN 201510582081 A CN201510582081 A CN 201510582081A CN 105119019 B CN105119019 B CN 105119019B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The present invention relates to a kind of electrolyte, including：Lithium salts, nonaqueous solvents and additive, described additive are a kind of cyclenes ester that logical formula (I) or logical formula (II) are represented, wherein, R1Represent one kind in alkyl phosphoric acid ester group, fluorinated phosphate ester group, phosphonitrile base, R2Represent the alkyl sulphonyl that alkoxy carbonyl or carbon number that alkyl or carbon number that carbon number is 1 12 are 1 12 are 1 12, or the alkenyl that carbon number is 1 12, and R2All hydrogen atoms are substituted with halogen atoms in substituent.The electrolyte can form stable interfacial film on both positive and negative polarity surface when lithium ion battery is made, suppress the reactivity of electrode surface, reduce the oxidation Decomposition of electrolyte, effectively suppress flatulence, so as to improve the security performance and cycle performance especially high temperature cyclic performance and service life under high voltages of lithium ion battery.
Description
Technical field
The present invention relates to technical field of chemical power, and in particular to one kind can take into account cycle performance of battery and fire resistance
Non-aqueous electrolyte for lithium ion cell, and using the electrolyte lithium ion battery.
Background technology
Compared with traditional secondary cell, lithium ion battery has operating voltage height, small volume, light weight, energy density
It is height, memory-less effect, pollution-free, and self discharge it is small, the advantages of have extended cycle life.Nineteen ninety, Japanese Sony companies produce
First piece of lithium ion battery, has started the commercialization tide of lithium ion battery.In recent years, lithium rechargeable battery is except applying
Consumer electronics product field, is also widely used on electric automobile, and is considered as solving automobile exhaust pollution, reduces fossil energy
The important means of source consumption.At present, one of development bottleneck of electric automobile is exactly that service life is short and safety risks, is reflected in
On battery, be exactly battery cycle performance is poor and poor safety performance.Research discovery, solvent during lithium cell charging in electrolyte
Occurs oxidation Decomposition in positive pole, catabolite hinders the electrochemical reaction desired by battery, therefore causes battery performance to decline.
In addition, during repeated charge, the solvent in electrolyte can also cause the decline of battery performance in the reduction decomposition of graphite cathode,
Decompose more serious particularly with the electrolyte oxidation of the materials such as high voltage nickel manganese, ternary, caused potential safety hazard is bigger.In order to carry
The cycle performance and security performance of lithium ion battery are risen, except seeking new positive and negative pole material, new electrolyte prescription is developed
It is also a kind of important solution.
Non-aqueous electrolyte for lithium ion cell is mainly dissolves what is formed in organic solvent by electrolyte lithium salt.In addition, electric
Solve and certain additive is also included in liquid, in the film forming, the electrical conductivity of lifting electrolyte, reduction battery for promoting graphite cathode
Resistance, the storge quality for improving battery, the cycle performance for lifting battery etc..
Because the energy density of LiFePO4 is relatively low, sight has been invested the higher ternary material of energy density, height by people
On voltage nickel manganese material and rich lithium material.But high voltage material makes the solvent in electrolyte occur to divide in charge and discharge process
Solution, so as to cause cycle performance poor, certain safety problem also occurs therewith.Current people's exploitation high-voltage electrolyte is mainly
Using the solvent of perfluoro.In order to reduce the combustibility of electrolyte, traditional method is that phosphorus system or halogen are added into electrolyte
Plain fire retardant.It is difficult while taking into account the high voltage capability and fire resistance of electrolyte using single adding method.
The content of the invention
The electrolyte of high voltage capability, cycle performance and security performance can be taken into account it is an object of the invention to provide a,
And the lithium ion battery containing the electrolyte.
In order to realize foregoing invention purpose, the technical solution adopted by the present invention is as follows：
A kind of electrolyte, including：Lithium salts, nonaqueous solvents and additive, it is characterised in that described additive is logical
A kind of cyclenes ester that formula (I) or logical formula (II) are represented, wherein, R1Represent in alkyl phosphoric acid ester group, fluorinated phosphate ester group, phosphonitrile base
One kind；R2Represent that alkoxy carbonyl or carbon number that alkyl or carbon number that carbon number is 1-12 are 1-12 are 1-
12 alkyl sulphonyl or carbon number is 1-12 alkenyl, and R2All hydrogen atoms are taken by halogen atom in substituent
Generation.
Preferably, electrolyte also includes vinylene carbonate, propylene sulfite, methane-disulfonic acid methylene ester, ethylene
One or more in alkene ethyl.
Preferably, the gross weight percentage composition of the additive in the electrolytic solution is 1%~10%.
Preferably, the gross weight percentage composition of the additive in the electrolytic solution is 1%~3%.
Preferably, in described electrolyte vinylene carbonate, propylene sulfite, methane-disulfonic acid methylene ester, carbon
The gross weight percentage composition of sour vinylethylene is 0%~5%.
Preferably, in described electrolyte vinylene carbonate, propylene sulfite, methane-disulfonic acid methylene ester, carbon
The gross weight percentage composition of sour vinylethylene is 1%~3%.
Preferably, a kind of lithium ion battery, including：Positive plate, negative plate, electrolyte and it is interval in adjacent positive/negative plate
Between barrier film, the electrolyte be above-mentioned electrolyte.
Preferably, the material of described positive plate is one kind in nickel manganese, ternary, lithium ferric manganese phosphate, the material of negative plate
For the one or more mixing in native graphite, Delanium, silicon-carbon, hard carbon, lithium titanate material.
The beneficial effects of the present invention are：
Electrolyte of the present invention shows good cycle performance, especially high temperature cyclic performance in high voltage material, together
When the electrolyte combustibility substantially reduce, have a larger raising to the security performance of battery.
Stable interfacial film, suppression can be formed when lithium ion battery is made using the electrolyte of the present invention on both positive and negative polarity surface
The reactivity of electrode surface processed, reduces the oxidation Decomposition of electrolyte, effectively suppresses flatulence, so as to improve lithium ion battery
Security performance and cycle performance especially high temperature cyclic performance and service life under high voltages.
Brief description of the drawings
Fig. 1 is 55 DEG C of high temperature circulation figures of embodiment 1 and comparative example 1；
Fig. 2 is 55 DEG C of high temperature circulation figures of embodiment 2 and comparative example 2；
Fig. 3 is SET (self-extinguishing time) figure under the methyl cyclenes ester various concentrations of 1,4 methyl orthophosphoric acid base of additive -2,3.
Embodiment
Below by embodiment, the present invention will be further described, but embodiment is not intended to limit protection scope of the present invention.
Embodiment 1
(1) electrolyte quota：According to EC：PC：DEC：EMC：VC：PS=35：5：35：25：2：2.5 (volume ratios) are prepared
1mol/L LiPF6Electrolyte, then adds Isosorbide-5-Nitrae methyl orthophosphoric acid base -2,3 methyl cyclenes ester of weight percentage 2%.
(2) preparation of positive electrode：The LiNi of mixed weight percentage composition 91%0.5Mn1.5O2(positive active material), weight
The SP (superconduction carbon black) of the percentage composition 4% and PVDF (binding agent) of weight percentage 5% is measured, and N- methyl is added to it
Slurry is made in pyrrolidones, and slurry is coated on aluminium foil, roll-in after drying, and obtains positive electrode.
(3) preparation of negative material：In the Delanium of mixed weight percentage composition 75%, weight percentage 20%
Between phase carbon microspheres, the sodium carboxymethylcellulose of weight percentage 5%, and to its add deionized water, then slurry is coated
On copper foil, roll-in after drying obtains negative material.
(4) by above-mentioned positive and negative pole material be prepared into 1865140 square battery (length, width and height be respectively 140mm, 65mm and
18mm), wherein, positive electrode compacted density be 2.17g/cm3, the thickness of pole piece is 162 μm (two-sided)；Negative material compacting is close
Spend 1.46g/cm3, the thickness of pole piece is 104 μm.
(5) above-mentioned battery is made to be melted into according to following techniques：(1) 260mA constant-current charges, pressure limiting 3.65V, in limited time 240min；
(2) 2600mA constant-current constant-voltage chargings, pressure limiting 3.65V, current limliting 200mA, in limited time 240min.Then according to 1C (13000mA) work
Skill carries out normal temperature circulation discharge and recharge；High temperature (55 DEG C) cycle charge-discharge is carried out according to 0.5C (6500mA), as a result shows, works as capacity
When decaying to the 80% of initial capacity, normal temperature circulation number of times is 600 weeks, and high temperature circulation number of times is 400 weeks, and high temperature cyclic performance is bright
Aobvious lifting, specific See Figure 1.
Embodiment 2
(1) electrolyte quota：According to EC：PC：DEC：EMC：VC：PS=35：5：35：25：2：2.5 (volume ratios) are prepared
1mol/L LiPF6Electrolyte, then adds Isosorbide-5-Nitrae methyl orthophosphoric acid base -2,3 methyl cyclenes ester of weight percentage 2.5%.
(2) preparation of positive electrode：Mix 72wt% LiNi1/3Co1/3Mn1/3O2And 18wt%LiMn0.8Fe0.2O4(just
Pole active material), the SP (superconduction carbon black) and the PVDF (binding agent) of weight percentage 5% of weight percentage 5%, and
1-METHYLPYRROLIDONE being added to it slurry being made, slurry is coated on aluminium foil, roll-in after drying obtains positive electrode.
(3) preparation of negative material：In the Delanium of mixed weight percentage composition 75%, weight percentage 20%
Between phase carbon microspheres, the sodium carboxymethylcellulose of weight percentage 5%, and to its add deionized water, then slurry is coated
On copper foil, roll-in after drying obtains negative material.
(4) by above-mentioned positive and negative pole material be prepared into 1865140 square battery (length, width and height be respectively 140mm, 65mm and
18mm), wherein, positive electrode compacted density be 3g/cm3, surface density is 170g/m2(one side)；Negative material compacted density
1.46g/cm3, the thickness of pole piece is 104 μm.
(5) above-mentioned battery is made to be melted into according to following techniques：(1) 200mA constant-current charges, pressure limiting 4.17V, in limited time 240min；
(2) 3000mA constant-current constant-voltage chargings, pressure limiting 4.17V, current limliting 200mA, in limited time 240min.Then according to 1C (15000mA) work
Skill carries out normal temperature circulation discharge and recharge；High temperature (55 DEG C) cycle charge-discharge is carried out according to 0.5C (7500mA), as a result shows, works as capacity
When decaying to the 80% of initial capacity, normal temperature circulation number of times is 2500 weeks, and high temperature circulation number of times is 800 weeks, high temperature cyclic performance
It is obviously improved, specific See Figure 2.
Embodiment 3
(1) configuration baseline electrolyte is according to EC：PC：DEC：EMC：VC：PS=35：5：35：25：2：2.5 (volume ratios) are matched somebody with somebody
1mol/L LiPF processed6Electrolyte, is then added to benchmark by Isosorbide-5-Nitrae methyl orthophosphoric acid base -2,3 methyl cyclenes ester with different concentration
In electrolyte (1%, 5%, 10%, 15%, 20%, 25%, 30%, 40%), it is well mixed, aforesaid operations are in argon gas gloves
Completed in case.
(2) electrolyte of the self-extinguishing time method to the above-mentioned methyl orthophosphoric acids of 1,4- containing various concentrations base -2,3 methyl cyclenes ester is utilized
Anti-flammability test is carried out, record test result See Figure 3 can be obtained, and with Isosorbide-5-Nitrae-methyl orthophosphoric acid base -2,-methyl cyclenes ester contains
The increase of amount, the self-extinguishing time of electrolyte shortens, and when being added to 25% and the above, electrolyte is completely non-ignitable.
Comparative example 1
(1) electrolyte quota：According to EC：PC：DEC：EMC：VC：PS=35：5：35：25：2：2.5 (volume ratios) are prepared
1mol/L LiPF6Electrolyte.
(2) preparation of positive electrode：The LiNi of mixed weight percentage composition 91%0.5Mn1.5O2(positive active material), weight
The SP (superconduction carbon black) of the percentage composition 4% and PVDF (binding agent) of weight percentage 5% is measured, and N- methyl is added to it
Slurry is made in pyrrolidones, and slurry is coated on aluminium foil, roll-in after drying, and obtains positive electrode.
(3) preparation of negative material：In the Delanium of mixed weight percentage composition 75%, weight percentage 20%
Between phase carbon microspheres, the sodium carboxymethylcellulose of weight percentage 5%, and to its add deionized water, then slurry is coated
On copper foil, roll-in after drying obtains negative material.
(4) by above-mentioned positive and negative pole material be prepared into 1865140 square battery (length, width and height be respectively 140mm, 65mm and
18mm), wherein, positive electrode compacted density be 2.17g/cm3, the thickness of pole piece is 162 μm (two-sided)；Negative material compacting is close
Spend 1.46g/cm3, the thickness of pole piece is 104 μm.
(5) above-mentioned battery is made to be melted into according to following techniques：(1) 260mA constant-current charges, pressure limiting 3.65V, in limited time 240min；
(2) 2600mA constant-current constant-voltage chargings, pressure limiting 3.65V, current limliting 200mA, in limited time 240min.Then according to 1C (13000mA) work
Skill carries out normal temperature circulation discharge and recharge；High temperature (55 DEG C) cycle charge-discharge is carried out according to 0.5C (6500mA), as a result shows, works as capacity
When decaying to the 80% of initial capacity, normal temperature circulation number of times is 400 weeks, and high temperature circulation number of times is 200 weeks.Normal temperature and high temperature circulation
Performance is not so good as embodiment 1.
Comparative example 2
(1) electrolyte quota：According to EC：PC：DEC：EMC：VC：PS=35：5：35：25：2：2.5 (volume ratios) are prepared
1mol/L LiPF6Electrolyte.
(2) preparation of positive electrode：The LiNi of mixed weight percentage composition 72%1/3Co1/3Mn1/3O2And 18wt%
LiMn0.8Fe0.2O4(positive active material), the SP (superconduction carbon black) of weight percentage 5% and weight percentage 5%
PVDF (binding agent), and slurry is made to its addition 1-METHYLPYRROLIDONE, slurry is coated on aluminium foil, roll-in after drying,
Obtain positive electrode.
(3) preparation of negative material：In the Delanium of mixed weight percentage composition 75%, weight percentage 20%
Between phase carbon microspheres, the sodium carboxymethylcellulose of weight percentage 5%, and to its add deionized water, then slurry is coated
On copper foil, roll-in after drying obtains negative material.
(4) by above-mentioned positive and negative pole material be prepared into 1865140 square battery (length, width and height be respectively 140mm, 65mm and
18mm), wherein, positive electrode compacted density be 3g/cm3, surface density is 170g/m2(one side)；Negative material compacted density
1.46g/cm3, the thickness of pole piece is 104 μm.
(5) above-mentioned battery is made to be melted into according to following techniques：(1) 200mA constant-current charges, pressure limiting 4.17V, in limited time 240min；
(2) 3000mA constant-current constant-voltage chargings, pressure limiting 4.17V, current limliting 200mA, in limited time 240min.Then according to 1C (15000mA) work
Skill carries out normal temperature circulation discharge and recharge；High temperature (55 DEG C) cycle charge-discharge is carried out according to 0.5C (7500mA), as a result shows, works as capacity
When decaying to the 80% of initial capacity, normal temperature circulation number of times is 2000 weeks, and high temperature circulation number of times is 450 weeks, and normal temperature and high temperature are followed
Ring performance is not so good as embodiment 2.
Table 1 gives the basic performance contrast of comparative example 1,2 and embodiment 1,2, therefrom it is seen that the addition of additive
Influence is not produced on its other performance.
The basic performance contrast table of table 1
| No. | Capacity (mAh) | Voltage (V) | Internal resistance (m Ω) | Normal temperature circulation | High temperature circulation |
| Embodiment 1 | 13428 | 4.712 | 7.956 | 600 weeks | 400 weeks |
| Comparative example 1 | 13400 | 4.705 | 7.999 | 400 weeks | 200 weeks |
| Embodiment 2 | 15250 | 4.009 | 5.05 | 2500 weeks | 800 weeks |
| Comparative example 2 | 15102 | 4.008 | 5.10 | 2000 weeks | 450 weeks |
Above-described embodiment is only example property.For those skilled in the art, it is possible to understand that do not departing from the present invention
Principle and spirit in the case of can to these embodiments carry out it is a variety of change, modification, replace and be denatured, the scope of the present invention
It is defined by the appended claims and the equivalents thereof.
Claims (8)
1. a kind of electrolyte, including：Lithium salts, nonaqueous solvents and additive, it is characterised in that described additive is Isosorbide-5-Nitrae phosphorus
The sour methyl of carbomethoxy -2,3 cyclenes ester.
2. electrolyte as claimed in claim 1, it is characterised in that electrolyte also includes vinylene carbonate, sulfurous acid propylene
One or more in ester, methane-disulfonic acid methylene ester, vinylethylene carbonate.
3. electrolyte as claimed in claim 1, it is characterised in that the gross weight percentage composition of the additive in the electrolytic solution
For 1%~10%.
4. electrolyte as claimed in claim 3, it is characterised in that the gross weight percentage composition of the additive in the electrolytic solution
For 1%~3%.
5. electrolyte as claimed in claim 2, it is characterised in that vinylene carbonate, sulfurous acid in described electrolyte
Weight percentage is 0% after one or more of solvent combinations in propylene, methane-disulfonic acid methylene ester, vinylethylene carbonate
~5%.
6. electrolyte as claimed in claim 5, it is characterised in that vinylene carbonate, sulfurous acid in described electrolyte
Weight percentage is 1% after one or more of solvent combinations in propylene, methane-disulfonic acid methylene ester, vinylethylene carbonate
~3%.
7. a kind of lithium ion battery, including：Positive plate, negative plate, electrolyte and be interval between adjacent positive/negative plate every
Film, it is characterised in that the electrolyte is the electrolyte any one of claim 1-6.
8. lithium ion battery as claimed in claim 7, it is characterised in that the material of described positive plate is nickel manganese, ternary, phosphorus
One kind in sour ferrimanganic lithium, the material of negative plate is one kind in native graphite, Delanium, silicon-carbon, hard carbon, lithium titanate material
Or several mixing.
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| FR3044830B1 (en) * | 2015-12-08 | 2020-06-12 | Commissariat A L'energie Atomique Et Aux Energies Alternatives | ELECTROCHEMICAL CELL FOR LITHIUM BATTERY COMPRISING A SPECIFIC ELECTROLYTE |
| CN107623142A (en) * | 2017-09-07 | 2018-01-23 | 山东鸿正电池材料科技有限公司 | A kind of high power lithium ion power battery |
| CN108807974B (en) * | 2018-06-29 | 2021-07-09 | 宁德时代新能源科技股份有限公司 | Lithium ion battery |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102610859A (en) * | 2012-04-04 | 2012-07-25 | 山东鸿正电池材料科技有限公司 | Non-aqueous electrolyte for lithium manganate power battery |
| CN102709589A (en) * | 2012-02-17 | 2012-10-03 | 深圳新宙邦科技股份有限公司 | Lithium ion battery and electrolyte thereof |
| CN103579676A (en) * | 2013-10-10 | 2014-02-12 | 珠海市赛纬电子材料有限公司 | Non-aqueous electrolyte for high-voltage lithium ion batteries |
| CN103972586A (en) * | 2013-01-28 | 2014-08-06 | 华为技术有限公司 | A non-aqueous organic electrolyte and preparation method thereof, and a lithium ion rechargeable battery |
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Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102709589A (en) * | 2012-02-17 | 2012-10-03 | 深圳新宙邦科技股份有限公司 | Lithium ion battery and electrolyte thereof |
| CN102610859A (en) * | 2012-04-04 | 2012-07-25 | 山东鸿正电池材料科技有限公司 | Non-aqueous electrolyte for lithium manganate power battery |
| CN103972586A (en) * | 2013-01-28 | 2014-08-06 | 华为技术有限公司 | A non-aqueous organic electrolyte and preparation method thereof, and a lithium ion rechargeable battery |
| CN103579676A (en) * | 2013-10-10 | 2014-02-12 | 珠海市赛纬电子材料有限公司 | Non-aqueous electrolyte for high-voltage lithium ion batteries |
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